Abstract

We report large third-order nonlinear optical susceptibilities ${\chi }_{\mathit{ijkl}}^{〈3〉}$ of new tetrathiafulvalene derivatives, using the degenerate four-wave mixing (DFWM) method. To understand the physical nature of the optical nonlinearities, we separate their electronic and nuclear contributions. The electronic contribution to the third-order nonlinear optical susceptibilities of the molecules turns out to be dominant. From DFWM measurements we also deduce the values of the second-order hyperpolarizabilities $\gamma$, which are $\sim {10}^5$ greater than the $\gamma$ value of ${\mathrm{CS}}_2$

© 1998 Optical Society of America

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